Polyzwitterion (polyZI) supported ionogel electrolytes have emerged as promising candidates for battery electrolyte applications. Recent experimental studies have demonstrated that zwitterionic (ZI) gel electrolytes – comprising polyzwitterion-supported ionic liquids doped with alkali metal salts – are instrumental in the decoupling mechanical stiffness from ionic conductivity. Our previous findings highlight the critical role of the alkali metal cation — zwitterionic polymer and alkali metal cation — common anion interactions in determining the dynamic and structural properties in the polyzwitterionic ionogels. However, the influence of polyzwitterionic chemistry on the properties of the polyZI ionogel electrolyte remains largely unexplored. In this study, we used atomistic molecular dynamic simulations to probe the impact of polyzwitterionic chemistries, specifically, carboxbetaine and phosphorylcholine chemistries, affect the ion transport properties in polyZI ionogels. Our results show that the polyzwitterion with the backbone – cationic moiety – anionic moiety architecture (carboxybetaine polyZI) exhibits slower conductivity compared to a polyzwitterion with the backbone – anionic moiety – cationic moiety arrangement (Phosphorylcholine polyZI). Lastly, we discuss guiding the polyZI ionogel designs based on our findings.
